Study of sulfur poisoning on Pd/Al2O3 and Pd/CeO2/Al2O3 methane combustion catalysts

被引:48
作者
Colussi, Sara [1 ]
Arosio, Fabrizio [2 ]
Montanari, Tania [3 ]
Busca, Guido [3 ]
Groppi, Gianpiero [2 ]
Trovarelli, Alessandro [1 ]
机构
[1] Univ Udine, Dipartimento Sci & Tecnol Chim, I-33100 Udine, Italy
[2] Politecn Milan, Dipartimento Energia, I-20133 Milan, Italy
[3] Univ Genoa, Dipartimento Ingn Chim & Proc, I-16145 Genoa, Italy
关键词
CH4; combustion; Pd catalysts; Cerium oxide; Sulfur poisoning; SUPPORTED PALLADIUM; OXIDATION CATALYST; LOW-TEMPERATURE; DEACTIVATION; ALUMINA; CERIA; AL2O3; WATER; CEO2; SO2;
D O I
10.1016/j.cattod.2009.02.019
中图分类号
O69 [应用化学];
学科分类号
081704 ;
摘要
In the present work the CH4 combustion behavior of Pd/Al2O3 and Pd/CeO2/Al2O3 catalysts in the presence of SO2 is investigated under various reaction conditions. Attention is paid also to the behavior of the bare supports without the active phase. Both fresh and poisoned samples are characterized by IR spectroscopy and in situ CO adsorption. Transient activity measurements after SO2 poisoning indicate that regardless of CeO2 loading a strong deactivation of all catalysts is observed compared to fresh samples. The effect of sulfur poisoning on steady state activity at 653 and 873 K is also measured. The deactivation is evident only at 653 K and its dynamics reflects the dynamics of SO2 adsorption. Results of TPD experiments under inert or reaction atmosphere suggest that the dynamics of SO2 desorption is influenced by the combustion reaction taking place on the catalyst active sites. Ceria-doped catalysts are more sensitive to the composition of the atmosphere of adsorption/desorption and quantitative measurements indicate that the presence of CeO2 inhibits SO2 adsorption under reaction conditions. (C) 2009 Elsevier B.V. All rights reserved.
引用
收藏
页码:59 / 65
页数:7
相关论文
共 41 条
[1]   Poisoning and deactivation of palladium catalysts [J].
Albers, P ;
Pietsch, J ;
Parker, SF .
JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL, 2001, 173 (1-2) :275-286
[2]   Effect of alternate CH4-reducing/lean combustion treatments on the reactivity of fresh and S-poisoned Pd/CeO2/Al2O3 catalysts [J].
Arosio, F. ;
Colussi, S. ;
Trovarelli, A. ;
Groppi, G. .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2008, 80 (3-4) :335-342
[3]   Regeneration of S-poisoned Pd/Al2O3 catalysts for the combustion of methane [J].
Arosio, F. ;
Colussi, S. ;
Groppi, G. ;
Trovarelli, A. .
CATALYSIS TODAY, 2006, 117 (04) :569-576
[4]   IMPACT OF SULFUR ON MODEL PALLADIUM-ONLY CATALYSTS UNDER SIMULATED 3-WAY OPERATION [J].
BECK, DD ;
SOMMERS, JW ;
DIMAGGIO, CL .
APPLIED CATALYSIS B-ENVIRONMENTAL, 1994, 3 (2-3) :205-227
[5]   Oxygen storage behavior of ceria-zirconia-based catalysts in the presence of SO2 [J].
Boaro, M ;
de Leitenburg, C ;
Dolcetti, G ;
Trovarelli, A ;
Graziani, M .
TOPICS IN CATALYSIS, 2001, 16 (1-4) :299-306
[6]   The effect of CeO2 on the dynamics of Pd-PdO transformation over Pd/Al2O3 combustion catalysts [J].
Colussi, Sara ;
Trovarelli, Alessandro ;
Groppi, Gianpiero ;
Llorca, Jordi .
CATALYSIS COMMUNICATIONS, 2007, 8 (08) :1263-1266
[7]   OXIDATION OF METHANE OVER SUPPORTED PRECIOUS METAL-CATALYSTS [J].
CULLIS, CF ;
WILLATT, BM .
JOURNAL OF CATALYSIS, 1983, 83 (02) :267-285
[8]   Influence of pretreatment atmosphere on the nature of silica-supported Pd generated via decomposition of Pd(acac)2:: an FTIR spectroscopic study of adsorbed CO [J].
Daniell, W ;
Landes, H ;
Fouad, NE ;
Knözinger, H .
JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL, 2002, 178 (1-2) :211-218
[9]   The activation of a Pd/γ-alumina catalyst during methane combustion:: investigation of the phenomenon and of potential causes [J].
Demoulin, O ;
Navez, M ;
Ruiz, P .
CATALYSIS LETTERS, 2005, 103 (1-2) :149-153
[10]   SULFUR POISONING, RECOVERY AND RELATED PHENOMENA OVER SUPPORTED PALLADIUM, RHODIUM AND IRIDIUM CATALYSTS FOR METHANE OXIDATION [J].
DENG, YQ ;
NEVELL, TG ;
EWEN, RJ ;
HONEYBOURNE, CL ;
JONES, MG .
APPLIED CATALYSIS A-GENERAL, 1993, 101 (01) :51-62